Theoretical study on the application of the largest aluminum-pyrazole ring in electrochemical nitrogen reduction reaction |
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| Institution: | 1. State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, China;2. School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China;3. Chinese Academy of Sciences, University of Chinese Academy of Sciences, Beijing 100049, China;4. Fujian College, University of Chinese Academy of Sciences, Fuzhou 350002, China;1. Institute for Sustainable Energy & College of Sciences, Shanghai University, Shanghai 200444, China;2. Key Laboratory for Advanced Technology in Environmental Protection of Jiangsu Province, Yancheng Institute of Technology, Yancheng 224051, China;3. State Key Laboratory of Advanced Special Steel & Shanghai Key Laboratory of Advanced Ferrometallurgy & School of Materials Science and Engineering, Shanghai University, Shanghai 200444, China.;1. School of Resources and Environment, University of Electronic Science and Technology of China, Chengdu 611731, China;2. Research Center for Carbon-Neutral Environmental & Energy Technology, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, China;1. School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013, China;2. School of Resource and Environmental Engineering, Jilin Institute of Chemical Technology, Jilin 132000, China;1. School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, China;2. School of Energy and Environment & Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong 999077, China |
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| Abstract: | Electrochemical nitrogen reduction reaction (NRR) is a mild and sustainable method for ammonia synthesis. Therefore, developing high activity, selectivity, and economic efficiency catalysts with considering the synergistic effects between catalysts and carriers to design novel structural models is very important. Considering the non-noble metal NRR catalyst, Mo3, we tried to find a suitable carrier which is stable and economical. Herein, we used the largest atomically precise aluminum-pyrazole ring (AlOC-69) to date (diameter up to 2.3 nm). The larger ring cavities and the presence of abundant hydroxy groups make AlOC-69 an ideal molecular carrier model and provide a basis for studying its structure-activity relationship. The formation energy (−0.76 eV) and stable Mo-O bonds indicate that Mo3 can be stabilized on the Al10O10 surface. Additionally, N2 has fully activated due to the strong interaction between the p-orbital of N and the d-orbital of Mo. The low limiting potential (−0.28 V) emerges that Mo3@Al10O10 has ideal catalytic activity and selectivity. This research provides a promising catalyst model and an understanding of its catalytic process at the atomic level, providing a new approach for the co-design of catalyst and carrier in NRR. |
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